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Hollow N-doped carbon spheres with anchored single-atom Fe sites for efficient electrocatalytic oxygen reduction

WANG Min-min FENG Chao LIU Yun-qi PAN Yuan

王敏敏, 冯超, 柳云骐, 潘原. 空心氮掺杂碳球锚定单原子铁位点用于高效电催化氧还原反应[J]. 燃料化学学报(中英文), 2023, 51(5): 581-588. doi: 10.1016/S1872-5813(22)60067-7
引用本文: 王敏敏, 冯超, 柳云骐, 潘原. 空心氮掺杂碳球锚定单原子铁位点用于高效电催化氧还原反应[J]. 燃料化学学报(中英文), 2023, 51(5): 581-588. doi: 10.1016/S1872-5813(22)60067-7
WANG Min-min, FENG Chao, LIU Yun-qi, PAN Yuan. Hollow N-doped carbon spheres with anchored single-atom Fe sites for efficient electrocatalytic oxygen reduction[J]. Journal of Fuel Chemistry and Technology, 2023, 51(5): 581-588. doi: 10.1016/S1872-5813(22)60067-7
Citation: WANG Min-min, FENG Chao, LIU Yun-qi, PAN Yuan. Hollow N-doped carbon spheres with anchored single-atom Fe sites for efficient electrocatalytic oxygen reduction[J]. Journal of Fuel Chemistry and Technology, 2023, 51(5): 581-588. doi: 10.1016/S1872-5813(22)60067-7

空心氮掺杂碳球锚定单原子铁位点用于高效电催化氧还原反应

doi: 10.1016/S1872-5813(22)60067-7
详细信息
  • 中图分类号: O643.3

Hollow N-doped carbon spheres with anchored single-atom Fe sites for efficient electrocatalytic oxygen reduction

Funds: The project was supported by National Natural Science Foundation of China (22108306), Taishan Scholars Program of Shandong Province (tsqn201909065) and Shandong Provincial Natural Science Foundation (ZR2021YQ15, ZR2020QB174).
More Information
  • 摘要: 本研究将单原子分散的Fe-N4位点锚定在氮掺杂空心多孔碳球上用于电催化氧还原反应,研究表明,所制备的Fe SAs/HNCSs-800催化剂表现出优异的电催化氧还原性能,其起始电位为0.925 V,半波电位为0.867 V。球差电镜和同步辐射X射线吸收光谱证实了催化剂中存在高度分散的Fe-N4单原子位点。通过密度泛函理论计算证明单原子Fe-N4位点是氧还原反应有效的活性位点,其相邻的C缺陷可以有效调控单原子Fe的电子结构,进而提高电催化氧还原性能。
  • FIG. 2287.  FIG. 2287.

    FIG. 2287.  FIG. 2287.

    Figure  1  Synthesis of Fe SAs/HNCSs-800 catalyst

    Figure  2  (a) XRD pattern and (b) TEM image of Fe SAs/HNCSs-800, with the inset showing a TEM image of the HNCSs, (c) TEM image of Fe SAs/HNCSs-800 after stability test, (d) AC-HAADF-STEM and (e) HAADF-STEM-EDS elemental mapping images of Fe SAs/HNCSs-800

    Figure  3  (a) Fe K-edge spectra, (b) FT k2-weighted EXAFS spectra, (c) EXAFS fitting in k-space, (d) EXAFS fitting in R-space of Fe SAs/HNCSs-800, and (e) wavelet transform plots of Fe foil, FeO, Fe2O3 and Fe SAs/HNCSs-800

    Figure  4  (a) LSV curves, (b) Tafel plots, (c) cyclic voltammetry (CV) curves, and (d) kinetic current density (jk) curves of Fe SAs/HNCSs; (e) jk at 0.85 V and E1/2 values; (f) LSV curves before and after 3000-cycle durability test, with the inset showing the i-t curves of Fe SAs/HNCSs-800 and 20% Pt/C

    Figure  5  LSV curves of Fe SAs/HNCSs catalysts at different rotation speeds and corresponding K-L plots

    Figure  6  ((a), (b)) theoretical models of FeN4 and FeN4-C, (c) charge density difference of FeN4-C, ((d), (e)) DOS diagrams of FeN4 and FeN4-C, (f) adsorption energy of O2 on different catalysts, ((g)–(i)) calculated Gibbs free energy profiles for different catalysts in 0.1 mol/L KOH

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出版历程
  • 收稿日期:  2022-08-19
  • 修回日期:  2022-09-19
  • 录用日期:  2022-10-09
  • 网络出版日期:  2022-10-31
  • 刊出日期:  2023-05-15

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